Cyclometalation of lanthanum(iii) based MOF for catalytic hydrogenation of carbon dioxide to formate
Journal article, 2020
The hydrogenation of carbon dioxide (CO2) to formic acid is of great importance due to its useful properties in the chemical industry. In this work, we have prepared a novel metal-organic framework (MOF), JMS-1, using bipyridyl dicarboxylate linkers, with molecular formula [La2(bpdc)3(DMF)3]n. Network analysis of JMS-1 revealed a new 7-connected topology (zaz). The MOF backbone of the activated phase (JMS-1a) was functionalized by cyclometalation using [RuCl2(p-cymene)]2 to produce Ru(ii)@JMS-1a. Both JMS-1a and Ru(ii)@JMS-1a were able to convert CO2 in the presence of hydrogen to formate. Ru(ii)@JMS-1a displayed outstanding conversion evidenced by a yield of 98% of formate under optimized conditions of total pressure 50 bar (CO2/H2 = 1 : 4, temperature 110 °C, time 24 h, 5 mmol KOH, 8 mL ethanol). This work is significant in providing new strategies of incorporating active catalytic centres in MOFs for efficient and selective conversion of CO2 to formate.
Potassium hydroxide
Carbon dioxide
Lanthanum compounds
Hydrogenation
Organometallics
Chemical industry
Carboxylation
Author
Piwai Tshuma
University of Johannesburg
Midlands State University
B. C. E. Makhubela
University of Johannesburg
Lars Öhrström
Chalmers, Chemistry and Chemical Engineering, Chemistry and Biochemistry
S. A. Bourne
University of Cape Town
Nabanita Chatterjee
University of Cape Town
Isaac N. Beas
Botswana Institute for Technology Research and Innovation
J. Darkwa
Botswana Institute for Technology Research and Innovation
University of Johannesburg
G. Mehlana
Midlands State University
RSC Advances
20462069 (eISSN)
Vol. 10 6 3593-3605Subject Categories
Chemical Process Engineering
Other Chemical Engineering
Organic Chemistry
DOI
10.1039/c9ra09938g